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Effective regeneration of thermally deactivated commercial V-W-Ti catalysts

Xuesong SHANG, Jianrong LI, Xiaowei YU, Jinsheng CHEN, Chi HE

《化学科学与工程前沿(英文)》 2012年 第6卷 第1期   页码 38-46 doi: 10.1007/s11705-011-1167-z

摘要: An effective method for the regeneration of thermally deactivated commercial monolith SCR catalysts was investigated. Two types of regenerated solutions, namely NH Cl (1 mol/L) and dilute H SO (0.5 mol/L), were employed to treat the used catalyst. The effects of temperature and the regeneration process on the structural and textural properties of the catalysts were determined by X-ray diffraction, scanning electron microscopy, N adsorption/desorption, elemental analysis and Fourier transform infrared spectroscopy. The results suggest that the anatase phase of the used catalyst is maintained after exposure to high temperatures. Some of the catalytic activity was restored after regeneration. The catalyst regenerated by aqueous NH Cl had a higher activity than that of the catalyst treated by dilute H SO . The main reason is that the NH generated from the decomposition of NH Cl at high temperatures can be adsorbed onto the catalyst which promotes the reaction. The aggregated V O were partially re-dispersed during the regeneration process, and the intrinsic oxidation of ammonia with high concentrations of O is a factor that suppresses the catalytic activity.

关键词: V2O5-WO3/TiO2 catalysts     thermal deactivation     regeneration     NH4Cl     dilute H2SO4 solution    

different acid anions on highly efficient Ce-based catalysts for selective catalytic reduction of NO with NH<sub>3sub>

《化学科学与工程前沿(英文)》 2023年 第17卷 第10期   页码 1399-1411 doi: 10.1007/s11705-023-2345-5

摘要: Three kinds of Ce-based catalysts (CePO4, CeVO4, Ce2(SO4)3) were synthesized and used for the selective catalytic reduction (SCR) of NO by NH3. NH3-SCR performances were conducted in the temperature range of 80 to 400 °C. The catalytic efficiencies of the three catalysts are as follow: CePO4 > CeVO4 > Ce2(SO4)3, which is in agreement with their abilities of NH3 adsorption capacities. The highest NO conversion rate of CePO4 could reach about 95%, and the catalyst had more than 90% NO conversion rate between 260 and 320 °C. The effect of PO43–, VO43– and SO42– on NH3-SCR performances of Ce-based catalysts was systematically investigated by the X-ray photoelectron spectroscopy analysis, NH3 temperature programmed desorption, H2 temperature programmed reduction and field emission scanning electron microscopy tests. The key factors that can enhance the SCR are the existence of Ce4+, large NH3 adsorption capacity, high and early H2 consumptions, and suitable microstructures for gas adsorption. Finally, CePO4 and CeVO4 catalysts also exhibited relatively strong tolerance of SO2, and the upward trend about 8% was detected due to the sulfation enhancement by SO2 for Ce2(SO4)3.

关键词: CePO4     CeVO4     Ce2(SO4)3     selective catalytic reduction     NO removal    

On the monolayer dispersion behavior of Co<sub>3sub>O<sub>4sub> on HZSM-5 support: designing applicable

《化学科学与工程前沿(英文)》 2023年 第17卷 第11期   页码 1741-1754 doi: 10.1007/s11705-023-2332-x

摘要: Based on monolayer dispersion theory, Co3O4/ZSM-5 catalysts with different loadings have been prepared for selective catalytic reduction of nitrogen oxides by ammonia. Co3O4 can spontaneously disperse on HZSM-5 support with a monolayer dispersion threshold of 0.061 mmol 100 m–2, equaling to a weight percentage around 4.5%. It has been revealed that the quantities of surface active oxygen (O2) and acid sites are crucial for the reaction, which can adsorb and activate NOx and NH3 reactants effectively. Below the monolayer dispersion threshold, Co3O4 is finely dispersed as sub-monolayers or monolayers and in an amorphous state, which is favorable to generate the two kinds of active sites, hence promoting the performance of ammonia selective catalytic reduction of nitrogen oxide. However, the formation of crystalline Co3O4 above the capacity is harmful to the reaction performance. 4% Co3O4/ZSM-5, the catalyst close to the monolayer dispersion capacity, possesses the most abundant active O2 species and acidic sites, thereby demonstrating the best reaction performance in all the samples. It is proposed the optimal Co3O4/ZSM-5 catalyst can be prepared by loading the capacity amount of Co3O4 onto HZSM-5 support.

关键词: Co3O4/ZSM-5     NOx-SCR by NH3     monolayer dispersion threshold effect     surface acid sites     surface active O2 anions    

Removal of ammonium and nitrate through Anammox and FeS-driven autotrophic denitrification

《环境科学与工程前沿(英文)》 2023年 第17卷 第6期 doi: 10.1007/s11783-023-1674-4

摘要:

● Simultaneous NH4+/NO3 removal was achieved in the FeS denitrification system

关键词: Anammox     Denitrification     FeS     NH4+/NO3     Sulfammox    

Phase equilibrium of the ternary system of NH 4 Cl—CaCl 2 —H 2 O at 50°C

Xia LI, Junsheng YUAN, Zhiyong JI, Jianxin CHEN,

《化学科学与工程前沿(英文)》 2010年 第4卷 第1期   页码 75-77 doi: 10.1007/s11705-009-0296-0

摘要: The equilibrium data on the ternary system of NHCl—CaCl—HO at 50°C were investigated using the wet-residue method. The experimental results show that there are three pure phase crystal areas of NHCl, 2NHCl·CaCl·3HO and CaCl·2HO, two mixture phase crystal areas of NHCl and 2NHCl·CaCl·3HO, and 2NHCl·CaCl·3HO and CaCl·2HO in the system. A new hydration double salt (2NHCl·CaCl·3HO) was found in the ternary equilibrium system for the first time.

Denitrification performance and sulfur resistance mechanism of Sm–Mn catalyst for low temperature NH-SCR

《化学科学与工程前沿(英文)》 2023年 第17卷 第5期   页码 617-633 doi: 10.1007/s11705-022-2258-8

摘要: MnOx and Sm–Mn catalysts were prepared with the coprecipitation method, and they showed excellent activities and sulfur resistances for the selective catalytic reduction of NOx by NH3 between 50 and 300 °C in the presence of excess oxygen. 0.10Sm–Mn catalyst indicated better catalytic activity and sulfur resistance. Additionally, the Sm doping led to multi-aspect impacts on the phases, morphology structures, gas adsorption, reactions process, and specific surface areas. Therefore, it significantly enhances the NO conversion, N2 selectivity, and sulfur resistance. Based on various experimental characterization results, the reaction mechanism of catalysts and the effect of SO2 on the reaction process about the catalysts were extensively explored. For 0.10Sm–Mn catalyst, manganese sulfate and sulfur ammonium cannot be generated broadly under the influence of SO2 and the amount of surface adsorbed oxygen. The Bronsted acid sites strengthen significantly due to the addition of SO2, enhancing the sulfur resistance of the 0.10Sm–Mn catalyst.

关键词: MnOx     Sm–Mn     catalyst     NH3-SCR     sulfur resistance    

CeO doping boosted low-temperature NH-SCR activity of FeTiO catalyst: A microstructure analysis and reaction

《环境科学与工程前沿(英文)》 2022年 第16卷 第5期 doi: 10.1007/s11783-022-1539-2

摘要:

• CeO2 doping significantly improved low-temperature NH3-SCR activity on FeTiOx.

关键词: NH3-SCR     CeO2 doping     Low-temperature NOx removal     Improved redox property     In situ XAFS analysis    

Enabling nickel ferrocyanide nanoparticles for high-performance ammonium ion storage

《化学科学与工程前沿(英文)》 2023年 第17卷 第2期   页码 226-235 doi: 10.1007/s11705-022-2198-3

摘要: Prussian blue and its analogs are extensively investigated as a cathode for ammonium-ion batteries. However, they often suffer from poor electronic conductivity. Here, we report a Ni2Fe(CN)6/multiwalled carbon nanotube composite electrode material, which is prepared using a simple coprecipitation approach. The obtained material consists of nanoparticles with sizes 30–50 nm and the multiwalled carbon nanotube embedded in it. The existence of multiwalled carbon nanotube ensures that the Ni2Fe(CN)6/multiwalled carbon nanotube composite shows excellent electrochemical performance, achieving a discharge capacity of 55.1 mAh·g–1 at 1 C and 43.2 mAh·g–1 even at 15 C. An increase in the ammonium-ion diffusion coefficient and ionic/electron conductivity based on kinetic investigations accounts for their high performance. Furthermore, detailed ex situ characterizations demonstrate that Ni2Fe(CN)6/multiwalled carbon nanotube composite offers three advantages: negligible lattice expansion during cycling, stable structure, and the reversible redox couple. Therefore, the Ni2Fe(CN)6/multiwalled carbon nanotube composite presents a long cycling life and high rate capacity. Finally, our study reports a desirable material for ammonium-ion batteries and provides a practical approach for improving the electrochemical performance of Prussian blue and its analogs.

关键词: nickel ferrocyanides     NH4+     electrochemistry     Prussian blue     aqueous ammonium ion batteries    

NH<sub>3sub>OH+/NH<sub>2sub>NH<sub>3sub>+作为B位阳离子的无金属六方钙钛矿含能材料 Article

尚宇, 余志鸿, 黄瑞康, 陈劭力, 刘德轩, 陈晓娴, 张伟雄, 陈小明

《工程(英文)》 2020年 第6卷 第9期   页码 1013-1018 doi: 10.1016/j.eng.2020.05.018

摘要: 文中通过合理地选择分子组分,经由易于规模放大的简单合成路线,以NH<sub>3sub>OH+NH<sub>2sub>NH<sub>3sub>+分别作为B位点阳离子构筑了两例无金属六方钙钛矿含能材料(H<sub>2sub>dabco)B(ClO<sub>4sub>)<sub>3sub>(分别命名为DAP-6和DAP-7,其中H<sub>2<与基于NH<sub>4sub>+阳离子构筑的立方钙钛矿类似物(H<sub>2sub>dabco)(NH<sub>4sub>)(ClO<sub>4sub>)<sub>特别地,DAP-7具有超高热稳定性(起始分解温度T<sub>dsub> = 375.3 °C)、高爆速(D = 8.883 km·ssp sub>= 265.3 s)均稍优于六硝基六氮杂异伍兹烷(CL-20:Q = 6.23 kJ·g‒1I<sub>sp

关键词: 含能材料     单质炸药     固体推进剂     无金属六方钙钛矿    

ZnFe<sub>2sub>O<sub>4sub>/BiVO<sub>4sub> Z-scheme heterojunction for efficient visible-light photocatalytic

《化学科学与工程前沿(英文)》 2023年 第17卷 第11期   页码 1728-1740 doi: 10.1007/s11705-023-2322-z

摘要: A novel Z-scheme ZnFe2O4/BiVO4 heterojunction photocatalyst was successfully synthesized using a convenient solvothermal method and applied in the visible light photocatalytic degradation of ciprofloxacin, which is a typical antibiotic contaminant in wastewater. The heterostructure of as-synthesized catalysts was confirmed using X-ray diffraction, scanning electron microscopy, transmission electron microscopy and X-ray photoelectron spectroscopy characterizations. Compared with the single-phase counterparts, ZnFe2O4/BiVO4 demonstrated considerably enhanced photogenerated charge separation efficiencies because of the Z-scheme transfer mechanism of electrons between the composite photocatalysts. Consequently, the 30% ZnFe2O4/BiVO4 catalyst afforded a degradation rate of up to 97% of 20 mg/L ciprofloxacin under 30 min of visible light irradiation with a total organic carbon removal rate of 50%, which is an excellent activity compared with ever reported BiVO4-based catalysts. In addition, the liquid chromatography-mass spectrometry and quantitative structure-activity relationships model analyses demonstrated that the toxicity of the intermediates was lower than that of the parent ciprofloxacin. Moreover, the as-synthesized ZnFe2O4/BiVO4 heterojunctions were quite stable and could be reused at least four times. This study thus provides a promising Z-scheme heterojunction photocatalyst for the efficient removal and detoxication of antibiotic pollutants from wastewater.

关键词: ZnFe2O4/BiVO4     Z-scheme heterojunction     photocatalytic degradation     ciprofloxacin    

Li<sub>4sub>SiO<sub>4sub>-coated LiNi<sub>0.5sub>Mn<sub>1.5sub>O<sub>4sub> as the high performance

Shifeng YANG, Wenfeng REN, Jian CHEN

《能源前沿(英文)》 2017年 第11卷 第3期   页码 374-382 doi: 10.1007/s11708-017-0494-2

摘要: The preparation of Li SiO -coated LiNi Mn O materials by sintering the SiO -coated nickel-manganese oxides with lithium salts using abundant and low-cost sodium silicate as the silicon source was reported. The samples were characterized by X-ray diffraction, scanning electron microscopy and transmission electron microscopy. It was found that a uniform and complete SiO coating layer could be obtained at a suitable pH value of 10, which transformed to a good Li SiO coating layer afterwards. When used as the cathode materials for lithium-ion batteries, the Li SiO -coated LiNi Mn O samples deliver a better electrochemical performance in terms of the discharge capacity, rate capability, and cycling stability than that of the pristine material. It can still deliver 111.1 mAh/g at 20 C after 300 cycles, with a retention ratio of 93.1% of the stable capacity, which is far beyond that of the pristine material (101.3 mAh/g, 85.6%).

关键词: lithium-ion batteries     cathode material     LiNi0.5Mn1.5O4     lithium-ion conductor     coating    

Rh<sub>2sub>O<sub>3sub>/hexagonal CePO<sub>4sub> nanocatalysts for N<sub>2sub>O decomposition

Huan Liu, Zhen Ma

《化学科学与工程前沿(英文)》 2017年 第11卷 第4期   页码 586-593 doi: 10.1007/s11705-017-1659-6

摘要: Hexagonal CePO nanorods were prepared by a precipitation method and hexagonal CePO nanowires were prepared by hydrothermal synthesis at 150 °C. Rh(NO ) was then used as a precursor for the impregnation of Rh O onto these CePO materials. The Rh O supported on the CePO nanowires was much more active for the catalytic decomposition of N O than the Rh O supported on CePO nanorods. The stability of both catalysts as a function of time on stream was studied and the influence of the co-feed (CO , O , H O or O /H O) on the N O decomposition was also investigated. The samples were characterized by N adsorption-desorption, inductively coupled plasma optical emission spectroscopy, X-ray diffraction, transmission electron microscopy, X-ray photoelectron microscopy, hydrogen temperature-programmed reduction, oxygen temperature-programmed desorption, and CO temperature-programmed desorption in order to correlate the physicochemical and catalytic properties.

关键词: Rh2O3     CePO4     N2O decomposition    

ZnFe<sub>2sub>O<sub>4sub> deposited on BiOCl with exposed (001) and (010) facets for photocatalyticreduction of CO<sub>2sub> in cyclohexanol

Guixian Song, Xionggang Wu, Feng Xin, Xiaohong Yin

《化学科学与工程前沿(英文)》 2017年 第11卷 第2期   页码 197-204 doi: 10.1007/s11705-016-1606-y

摘要: ZnFe O -BiOCl composites were prepared by both hydrothermal and direct precipitation processes and the structures and properties of the samples were characterized by various instrumental techniques. The samples were then used as catalysts for the photocatalytic reduction of CO in cyclohexanol under ultraviolet irradiation to give cyclohexanone (CH) and cyclohexyl formate (CF). The photocatalytic CO reduction activities over the hydrothermally prepared ZnFe O -BiOCl composites were higher than those over the directly-precipitated composites. This is because compared to the direct-precipitation sample, the ZnFe O nanoparticles in the hydrothermal sample were smaller and more uniformly distributed on the surface of BiOCl and so more heterojunctions were formed. Higher CF and CH yields were obtained for the pure BiOCl and BiOCl composite samples with more exposed (001) facets than for the samples with more exposed (010) facets. This is due to the higher density of oxygen atoms in the exposed (001) facets, which creates more oxygen vacancies, and thereby improves the separation efficiency of the electron-hole pairs. More importantly, irradiation of the (001) facets with ultraviolet light produces photo-generated electrons which is helpful for the reduction of CO to ·CO . The mechanism for the photocatalytic reduction of CO in cyclohexanol over ZnFe O -BiOCl composites with exposed (001) facets involves electron transfer and carbon radical formation.

关键词: reduction of CO2     cyclohexanol     ZnFe2O4 deposited BiOCl     facet     composite photocatalyst    

NO hydrogenation to NH over FeCu/TiO catalyst with improved activity

《化学科学与工程前沿(英文)》 2023年 第17卷 第12期   页码 1973-1985 doi: 10.1007/s11705-023-2364-2

摘要: Ammonia is crucial in industry and agriculture, but its production is hindered by environmental concerns and energy-intensive processes. Hence, developing an efficient and environmentally friendly catalyst is imperative. In this study, we employed a straightforward and efficient impregnation technique to create various Cu-doped catalysts. Notably, the optimized 10Fe-8Cu/TiO2 catalyst exhibited exceptional catalytic performance in converting NO to NH3, achieving an NO conversion rate exceeding 80% and an NH3 selectivity exceeding 98% at atmospheric pressure and 350 °C. We employed in situ diffuse reflectance Fourier transform infrared spectroscopy and conducted density functional theory calculations to investigate the intermediates and subsequent adsorption. Our findings unequivocally demonstrate that Cu doping enhances the rate-limiting hydrogenation step and lowers the energy barrier for NH3 desorption, thereby resulting in improved NO conversion and enhanced selectivity toward ammonia. This study presents a pioneering approach toward energy-efficient ammonia synthesis and recycling of nitrogen sources.

关键词: NO hydrogenation     synthetic ammonia     10Fe-xCu/TiO2     high selectivity    

Characterization and performance of V

Caiting LI, Qun LI, Pei LU, Huafei CUI, Guangming ZENG

《环境科学与工程前沿(英文)》 2012年 第6卷 第2期   页码 156-161 doi: 10.1007/s11783-010-0295-x

摘要: A series of CeO supported V O catalysts with various loadings were prepared with different calcination temperatures by the incipient impregnation. The catalysts were evaluated for low temperature selective catalytic reduction (SCR) of NO with ammonia (NH ). The effects of O and SO on catalytic activity were also studied. The catalysts were characterized by specific surface areas (S ) and X–ray diffraction (XRD) methods. The experimental results showed that NO conversion changed significantly with the different V O loading and calcination temperature. With the V O loading increasing from 0 to 10 wt%, NO conversion increased significantly, but decreased at higher loading. The optimum calcination temperature was 400°C. The best catalyst yielded above 80% NO conversion in the reaction temperature range of 160°C–300°C. The formation of CeVO on the surface of catalysts caused the decrease of redox ability.

关键词: V2O5/CeO2 catalysts     NH3-SCR (selective catalytic reduction)     the incipient impregnation     low temperatures    

标题 作者 时间 类型 操作

Effective regeneration of thermally deactivated commercial V-W-Ti catalysts

Xuesong SHANG, Jianrong LI, Xiaowei YU, Jinsheng CHEN, Chi HE

期刊论文

different acid anions on highly efficient Ce-based catalysts for selective catalytic reduction of NO with NH<sub>3sub>

期刊论文

On the monolayer dispersion behavior of Co<sub>3sub>O<sub>4sub> on HZSM-5 support: designing applicable

期刊论文

Removal of ammonium and nitrate through Anammox and FeS-driven autotrophic denitrification

期刊论文

Phase equilibrium of the ternary system of NH 4 Cl—CaCl 2 —H 2 O at 50°C

Xia LI, Junsheng YUAN, Zhiyong JI, Jianxin CHEN,

期刊论文

Denitrification performance and sulfur resistance mechanism of Sm–Mn catalyst for low temperature NH-SCR

期刊论文

CeO doping boosted low-temperature NH-SCR activity of FeTiO catalyst: A microstructure analysis and reaction

期刊论文

Enabling nickel ferrocyanide nanoparticles for high-performance ammonium ion storage

期刊论文

NH<sub>3sub>OH+/NH<sub>2sub>NH<sub>3sub>+作为B位阳离子的无金属六方钙钛矿含能材料

尚宇, 余志鸿, 黄瑞康, 陈劭力, 刘德轩, 陈晓娴, 张伟雄, 陈小明

期刊论文

ZnFe<sub>2sub>O<sub>4sub>/BiVO<sub>4sub> Z-scheme heterojunction for efficient visible-light photocatalytic

期刊论文

Li<sub>4sub>SiO<sub>4sub>-coated LiNi<sub>0.5sub>Mn<sub>1.5sub>O<sub>4sub> as the high performance

Shifeng YANG, Wenfeng REN, Jian CHEN

期刊论文

Rh<sub>2sub>O<sub>3sub>/hexagonal CePO<sub>4sub> nanocatalysts for N<sub>2sub>O decomposition

Huan Liu, Zhen Ma

期刊论文

ZnFe<sub>2sub>O<sub>4sub> deposited on BiOCl with exposed (001) and (010) facets for photocatalyticreduction of CO<sub>2sub> in cyclohexanol

Guixian Song, Xionggang Wu, Feng Xin, Xiaohong Yin

期刊论文

NO hydrogenation to NH over FeCu/TiO catalyst with improved activity

期刊论文

Characterization and performance of V

Caiting LI, Qun LI, Pei LU, Huafei CUI, Guangming ZENG

期刊论文